Lithium-ion intercalation by coupled ion-electron transfer
The underlying reaction mechanism in lithium-ion batteries remains poorly understood. We provide experimental and theoretical evidence that lithium intercalation occurs by coupled ion-electron transfer, where ion transfer across the electrode-electrolyte interface is facilitated by electron transfer to a neighboring redox site. Electrochemical measurements for a variety of common electrode and electrolyte materials reveal a universal dependence of the (de-)intercalation rate on Li<sup>+</sup> vacancy fraction, as well as temperature and electrolyte effects consistent with the theory, which could be used to guide the molecular design of lithium-ion battery interfaces.
Authors
- Tao Gao (ORCID: https://orcid.org/0000-0003-0204-3269)
- Debbie Zhuang (ORCID: https://orcid.org/0000-0002-1855-3768)
- Livia Giordano (ORCID: https://orcid.org/0000-0002-6879-9424)
- Dimitrios Fraggedakis (ORCID: https://orcid.org/0000-0003-3301-6255)
- Armando R.C. Neto
- Yash Samantaray (ORCID: https://orcid.org/0000-0002-9141-6305)
- Cristina Grosu (ORCID: https://orcid.org/0000-0002-3690-0460)
- Botao Huang (ORCID: https://orcid.org/0000-0001-5634-5620)
- Yun Zhu (ORCID: https://orcid.org/0000-0003-3884-4359)
- Ryoichi Tatara (ORCID: https://orcid.org/0000-0002-8148-5294)
- Shakul Pathak
- Martin Z. Bazant (ORCID: https://orcid.org/0000-0002-8200-4501)
- Yirui Zhang (ORCID: https://orcid.org/0000-0001-7604-8623)
- Harsh Agarwal (ORCID: https://orcid.org/0000-0002-5237-4819)
- Ryan Stephens
- Sravani R. Duggirala
- Yang Shao‐Horn (ORCID: https://orcid.org/0000-0001-8714-2121)
Institutions
- Shell (United States) (US)
- Massachusetts Institute of Technology (US)
- Columbia University (US)
- Shell (Netherlands) (NL)
Publication Details
- Journal
- Science
- Published
- 2025-10-02
- DOI
- https://doi.org/10.1126/science.adq2541
- Citations
- 24
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 17.53